Catalytic upgrading of bio-ethanol to 1,3-butadiene(1,3-BD,ETB)is a renewable and low-carbon technology for the bulk chemical production.Exploring robust catalysts and getting in-depth understanding of the relationshi...Catalytic upgrading of bio-ethanol to 1,3-butadiene(1,3-BD,ETB)is a renewable and low-carbon technology for the bulk chemical production.Exploring robust catalysts and getting in-depth understanding of the relationship between the structure of catalytic sites and reaction selectivity are of great significance for ETB process applications.In this study,we constructed a robust Cu-Zr/SiO_(2) catalyst by an ammonia evaporation and post-impregnation method.Over the optimal 2%Cu-8%Zr/SiO_(2) catalyst,superior performance of 69.6%1,3-BD selectivity and 71.2%ethanol conversion were obtained.Systematic characterizations revealed that three types of Cu-Zr-Si active sites were probably constructed on the Cu-8%Zr/SiO_(2) catalysts as varying the Cu loadings from 0.5 to 20%,affording greatly different activity and selectivity in the ETB process.The 1,3-BD productivity over the(SiO)_(2)(CuO)Zr-OH sites was 8.2 and 77.2 times higher than that of(CuO)_(2)-Zr-(OSi)2 and Cu-(O)_(2)-Zr-(OSi)2 sites,respectively,attributed to the high activities and good balance among the reactions of dehydrogenation,aldol condensation,and MPVO reduction.展开更多
基金supported by the National Natural Science Foundation of China(21721004,22108274)“Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of the Chinese Academy of Sciences(XDA 21060200).
文摘Catalytic upgrading of bio-ethanol to 1,3-butadiene(1,3-BD,ETB)is a renewable and low-carbon technology for the bulk chemical production.Exploring robust catalysts and getting in-depth understanding of the relationship between the structure of catalytic sites and reaction selectivity are of great significance for ETB process applications.In this study,we constructed a robust Cu-Zr/SiO_(2) catalyst by an ammonia evaporation and post-impregnation method.Over the optimal 2%Cu-8%Zr/SiO_(2) catalyst,superior performance of 69.6%1,3-BD selectivity and 71.2%ethanol conversion were obtained.Systematic characterizations revealed that three types of Cu-Zr-Si active sites were probably constructed on the Cu-8%Zr/SiO_(2) catalysts as varying the Cu loadings from 0.5 to 20%,affording greatly different activity and selectivity in the ETB process.The 1,3-BD productivity over the(SiO)_(2)(CuO)Zr-OH sites was 8.2 and 77.2 times higher than that of(CuO)_(2)-Zr-(OSi)2 and Cu-(O)_(2)-Zr-(OSi)2 sites,respectively,attributed to the high activities and good balance among the reactions of dehydrogenation,aldol condensation,and MPVO reduction.
